The CW-EPR Capabilities of a Dual DNP/EPR Spectrometer Operating at 14 and 7 T.

High-field electron paramagnetic resonance (EPR) measurements are indispensable for a better understanding of dynamic nuclear polarization (DNP), which relies on polarization transfer between electron and nuclear spins. DNP experiments are typically performed at high > 7 T magnetic fields and low ≤ 100 K temperatures, while EPR instrumentation capable of EPR measurements under these conditions is scarce. In this paper, we describe the CW EPR capabilities of a dual DNP/EPR spectrometer that is designed to carry out EPR experiments under "DNP conditions" at 14 and 7 T. In the first part, we present the design of this instrument, highlighting the choices made to allow for both DNP and EPR operations. The spectrometer uses a sweepable cryogen-free magnet with NMR-grade homogeneity, a closed-cycle cooling system, a quasi-optical induction mode bridge, and a superheterodyne receiver system. The probe design is optimized for low heat load and fast sample exchange under cryogenic conditions. The spectrometer can operate in frequency and field sweep modes, including wide field sweeps using the main coil of the magnet. In the second part, we present EPR spectra acquired over a wide range of samples and operating conditions, illustrating the CW EPR capabilities of the instrument.

Photovoltage and Photocurrent Absorption Spectra of Sulfur Vacancies Locally Patterned in Monolayer MoS2.

We report on the optical absorption characteristics of selectively positioned sulfur vacancies in monolayer MoS2, as observed by photovoltage and photocurrent experiments in an atomistic vertical tunneling circuit at cryogenic and room temperature. Charge carriers are resonantly photoexcited within the defect states before they tunnel through an hBN tunneling barrier to a graphene-based drain contact. Both photovoltage and photocurrent characteristics confirm the optical absorption spectrum as derived from ab initio GW and Bethe-Salpeter equation approximations. Our results reveal the potential of single-vacancy tunneling devices as atomic-scale photodiodes.

Bright excitonic multiplexing mediated by dark exciton transition in two-dimensional TMDCs at room temperature.

2D-semiconductors with strong light-matter interaction are attractive materials for integrated and tunable optical devices. Here, we demonstrate room-temperature wavelength multiplexing of the two-primary bright excitonic channels (Ab-, Bb-) in monolayer transition metal dichalcogenides (TMDs) arising from a dark exciton mediated transition. We present how tuning dark excitons via an out-of-plane electric field cedes the system equilibrium from one excitonic channel to the other, encoding the field polarization into wavelength information. In addition, we demonstrate how such exciton multiplexing is dictated by thermal-scattering by performing temperature dependent photoluminescence measurements. Finally, we demonstrate experimentally and theoretically how excitonic mixing can explain preferable decay through dark states in MoX2 in comparison with WX2 monolayers. Such field polarization-based manipulation of excitonic transitions can pave the way for novel photonic device architectures.